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Area of Science:

  • Condensed matter physics
  • Materials science
  • Physical chemistry

Background:

  • Amorphous solid water is crucial for understanding water's phase diagram.
  • X-ray scattering techniques, including XPCS, are vital for studying water's structure and dynamics.
  • Modern synchrotron and XFEL facilities enable simultaneous structural and dynamic investigations.

Purpose of the Study:

  • To investigate the non-equilibrium dynamics of high-density amorphous (HDA) ice during heating.
  • To characterize the structural transition from HDA to low-density amorphous (LDA) ice using X-ray scattering.
  • To analyze transition dynamics at various length scales using ultra-small angle X-ray scattering (USAXS).

Main Methods:

  • Utilized X-ray photon correlation spectroscopy (XPCS) to probe dynamics.
  • Employed wide-angle X-ray scattering (WAXS) to monitor structural transitions.
  • Applied a novel sample preparation technique for studying μm-sized ice layers.
  • Performed XPCS in an ultra-small angle (USAXS) geometry for length scales of 60 nm–800 nm.

Main Results:

  • Observed a clear separation into three dynamical regimes during the HDA-LDA transition.
  • Identified distinct dynamical crossovers at different length scales for the HDA-LDA transition.
  • Found that crystallization from LDA occurs homogeneously across the studied length scales.

Conclusions:

  • The HDA-LDA transition exhibits complex, length-scale-dependent dynamics.
  • Crystallization from LDA is a more uniform process compared to the HDA-LDA transformation.
  • XPCS and USAXS are powerful tools for characterizing non-equilibrium dynamics in amorphous ice.